A graphite oxide (GO) layer with ordered ultrafine TiO2 particles was synthesized using an ambient heterogeneous spark and the resulting materials displayed enhanced photocatalytic activity for hydrogen production. The ability of the TiO2@GO nanocomposites to produce hydrogen was significantly greater than that of spark-produced TiO2 particles, and even of p25-TiO2 and p25-TiO2@large reduced graphene oxide (LrGO). Even though nanoscale rGO hybridization with TiO2 nanoparticles resulted in the highest performance in hydrogenation, this ambient plasma synthesis of TiO2@GO composites nevertheless did make an appropriate structure for the photocatalytic performance comparable to that of p25-TiO2@LrGO without individual chemical preparation of rGO.